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Ferroelectricity, especially in hafnia-based thin films at nanosizes, hasbeen rejuvenated in the fields of low-power, nonvolatile and Si-compatiblemodern memory and logic applications. Despite tremendous efforts to explore theformation of the metastable ferroelectric phase and the polarizationdegradation during field cycling, the ability of oxygen vacancy to exactlyengineer and switch polarization remains to be elucidated. Here we reportreversibly electrochemical control of ferroelectricity inHf$_{0.5}$Zr$_{0.5}$O$_2$ (HZO) heterostructures with a mixed ionic-electronicLaSrMnO$_3$ electrode, achieving a hard breakdown field more than 18 MV/cm,over fourfold as high as that of typical HZO. The electrical extraction andinsertion of oxygen into HZO is macroscopically characterized and atomicallyimaged in situ. Utilizing this reversible process, we achieved multiplepolarization states and even repeatedly repaired the damaged ferroelectricityby reversed negative electric fields. Our study demonstrates the robust andswitchable ferroelectricity in hafnia oxide distinctly associated with oxygenvacancy and opens up opportunities to recover, manipulate, and utilize richferroelectric functionalities for advanced ferroelectric functionality toempower the existing Si-based electronics such as multi-bit storage.

Electrochemical control of ferroelectricity in hafnia-based ferroelectric devices using reversible oxygen migration